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com

25 29 August 2012, Prague, Czech Republic

fluidized bed reactors: The SMR and SE-SMR processes

J. Solsvik a*, Z. Chao, H. A. Jakobsen

Department of Chem. Eng., Norwegian University of Science and Technology (NTNU), Sem Slands vei 4, N-7491 Trondheim,

Norway

Abstract

A one-dimensional two-fluid EulerianEulerian model is adopted for numerical simulations of gassolid flows in

fluidized bed reactors. The simulation results obtained with the one-dimensional model are compared with the results

of a two-dimensional model for the SMR and SE-SMR processes. For the species concentrations and temperature

predictions, the one-dimensional and two-dimensional models are in good agreement. Deviations in the simulation

results are observed between the models in the phase area fractions and gas phase velocity. The one-dimensional

model should therefore be further extended to include the effect of the gas bubbles in the dense bed zone. Moreover,

it is necessary to compensate for the radial convective flow pattern by extended conductive fluxes.

2012 Published by Elsevier Ltd. Selection under responsibility of the Congress Scientific Committee

(Petr Kluson) Open access under CC BY-NC-ND license.

Keywords: SE-SMR; SMR; fluidized bed; two-fluid model; CO2-capture; numerical simulation

1. Introduction

Steam methane reforming (SMR) is currently the predominant industrial route for hydrogen

production. The development of alternative concepts for production of hydrogen via SMR has attracted a

lot of attention. A novel concept is the sorption-enhanced steam methane reforming (SE-SMR) process,

which involves the addition of a solid sorbent into the SMR reaction system for the selective removal of

* Corresponding author.

E-mail address: jannike.solsvik@chemeng.ntnu.no

1877-7058 2012 Published by Elsevier Ltd. Open access under CC BY-NC-ND license.

doi:10.1016/j.proeng.2012.07.419

284 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

Nomenclature

Latin Letters

Cp Heat capacity

D Diffusion coefficient

d Diameter

G Modulus of elasticity

g Gravity

h Heat transfer coefficient

H Tube height

H Heat of reaction

kk Thermal conductivity of phase k

% Interfacial drag force

p Pressure

i

Q Interfacial heat transfer

Ri Reaction rate of reaction i

Rj Formation rate of component j

T Temperature

t Time

v Velocity

w Weighting function

z Axial reactor dimension

Greek Letters

Sorbent-to-catalyst ratio

Inter-phase drag coefficient

Area phase fraction

Interfacial mass flux

Shear stress

Dynamic viscosity

Density

Mass fraction

J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294 285

Subscript

g Gas phase

i Reaction number

j Species type

k Phase (k=g,s)

mf minimum fluidization

p Particle

s Solid phase

t Tube

Superscript

Cap CO2 capture reaction

eff Effective

in Inlet, i.e. z = 0

m Molecular

out Outlet, i.e. z = H

s Superficial

SMR Reactions of steam methane reforming

T Turbulent

CO2; and thereby, shifting the equilibrium toward increased hydrogen production. A regeneration step

where the CO2 is released from the sorbent; and thus re-introduce the capture activity, is necessary to

make the SE-SMR process economically viable. Hence, the characteristic sorbent reactant utilized in the

SE-SMR processes must be exposed to different reactor operation conditions in a cyclic manner. The SE-

SMR process thus consists of two main steps: (i) reforming and (ii) regeneration. Because of the

heterogeneous nature of the SE-SMR reactions and the relatively short chemical activity life-time of the

sorbent, the circulating fluidized bed is a suitable reactor concept that provides possible continuous

operation of the process where the solid flux circulating between the reformer and regenerator reactor

units aims to successively recover and utilize the chemical activity of the sorbent.

Mathematical modeling and simulations of the SE-SMR process operated in fluidized bed reactors

have been performed ranging from the simpler Kunii-Levenspiel type models [1] to rigorous two-fluid

models based on kinetic theory of granular flows (KTGF) [25]. Adopting a Kunii-Levenspiel type of

model [6] the solids are commonly assumed to be stagnant in the reactor. Moreover, considering the

circulating fluidized bed design, a prescribed inter-transferred solid flux between the reactor units is

required. The SE-SMR process is dynamic in nature as the solid density and thus the flow behaviour like

the solid flux changes with time and reaction performance. Hence, the Kunii-Levenspiel models are not

appropriate to describe dynamic processes such as the SE-SMR technology. On the other hand, the two-

fluid EulerianEulerian models [7] treat the gas and solid particles as inter-penetrating continuous fluids.

Hence, a solid flux is incorporated in the two-fluid model which allows for dynamic modeling of

interconnected fluidized bed reactors. Lun et al. [8] and Gidaspow [9] have derived KTGF models which

286 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

have been widely adopted for modeling and simulation of fluidized bed reactors, e.g. the cold-flow

studies of Lindborg et al. [10] and Wang et al. [11]

Two- and three dimensional two-fluid models are yet too computational demanding due to the

complexity of the gassolid flow in the fluidized bed reactors. Moreover, chemical reactions and the

handling of large geometries of commercial reactors challenge the presently available computing

capacity. In particular, the computations becomes excessively time consuming for the additional

consideration of interconnected reactors in a circulating fluidized bed design because the dynamic solid

fluxes exchanging between the fluidized bed reactors needs to be incorporated in the numerical solution

algorithm. Such simulations are highly relevant and important in the progress of commercial fluidized bed

reactors for processes such as the novel SE-SMR technology. A one-dimensional two-fluid model has the

advantages of considerable lower computational costs relative to the two- and three dimensional models.

Whereas details; such as the bubble wakes and multidimensional flow phenomena like circulation cells or

vortices, in the complex gas-solid flow within a fluidized bed reactor is averaged out and lost with a one-

dimensional model, the chemical reactor performance and the important solid fluxes transferred between

the reactors in a interconnected fluidized bed design, may be accurately predicted by a one-dimensional

model.

In the present study, a one-dimensional two-fluid gassolid model is adopted for numerical simulation

of the SMR and SE-SMR processes. The simulation results obtained with the one-dimensional model are

compared with the results of a two-dimensional model. The present validation study of the one-

dimensional model is performed to elucidate whether the model can be reasonably adopted for further

simulations of interconnected fluidized bed reactors with a dynamic solid flux transferred between the

reactor units. Dynamic solid circulation between fluidized bed units that operate at different conditions is

an inherent requirement for the novel SE-SMR technology operated in fluidized bed reactors. A less

computational demanding one-dimensional model to study the performance of interconnected reactor

units will be an important contribution to the progress of the commercialization of circulating fluidized

bed reactors intended for the SE-SMR technology.

The SE-SMR process can be operated using either a combined catalyst/sorbent pellet design unifying

the catalytic and capture properties in a single pellet [1214], or separate the catalytic and capture

properties into two different pellet types. For simulation studies of the SE-SMR process using the two-

pellet design, a multi-fluid Eulerian model may be derived giving the possibility for a catalyst phase,

sorbent phase and gas phase; e.g., the cold flow model of Chao et al. [15] and the SE-SMR study by

Carlo et al. [16]. Recently, Solsvik and Jakobsen [17] and Rout et al. [18] performed a numerical study of

a pellet holding both catalytic and capture properties with the objective to investigate the SE-SMR

process. With this pellet design the Eulerian model holds a single solid phase that interpenetrates with the

gas phase. Rout and Jakobsen [19] extended the pellet study adopting the novel pellet design in fixed

packed bed simulations. In the present study, the one-pellet design is adopted.

2. Chemical reactions

The conventional SMR reactor utilizes a nickel-based catalyst to produce synthesis gas from a high-

temperature mixture of methane and steam. The reforming reactions (1) and (2), and the watergas-shift

reaction (3) are the most important reactions when converting methane in the presence of steam. When a

Ca-based sorbent is integrated in the SMR process, the presumable selective removal of CO2 is

represented by reaction (4).

J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294 287

CH 4 + 2H 2 O = CO 2 + 4H 2 H 298 = 164.7 kJ/mol (2)

CO + H 2 O = CO 2 + H 2 H 298 = 41.5 kJ/mol (3)

CO 2 + CaO = CaCO3 H 298 = 178 kJ/mol (4)

In this study, the reaction kinetic model of the reforming and shift reactions by Xu and Froment [20]

and the CO2 capture for dolomite sorbents by Sun et al. [21] were adopted.

3. Two-phase model

In the present study, a one-dimensional two-fluid EulerianEulerian model describing gassolid flows

with the complexity of chemical reactions in fluidized bed reactors is derived. The governing equations

are presented by relations (5) to (10) and the constitutive equations are presented in Appendix A. Further

details on the constitutive equations and the numerical solution algorithm using the finite volume method

[2223] are given by Lindborg [24].

Continuity equation for phase k (=g,s):

(k k ) + (k k vk ) = k (5)

t z

pg 4g g ,wall g

(g g vg ) + (g g vg vg ) = g + + g g g z + %g (6)

t z z dt z

pg 4s s ,wall s

(s s vs ) + (s s vs vs ) = s + + s s g z G (g ) s + %s (7)

t z z dt z z

(k k k , j ) + (k k vk k , j ) = (k k Dkeff, j k , j ) + Rk , j (8)

t z z z

Tg Tg T

g g Cpg + g g Cpg vg = (g k geff g ) + ( H iSMR )RiSMR + Qgi (9)

t z z z i

288 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

Ts T T

s s Cps + s s Cps vs s = (s kseff s ) + (H Cap ) R Cap Qgi (10)

t z z z

An in-house code for a one-dimensional two-fluid EulerianEulerian model has been developed for

fluidized bed reactors. The one-dimensional model has been applied to simulate the SMR and SE-SMR

processes and the results have been compared with the results of a two-dimensional model. A cross-

sectional averaging operator is adopted to present the results of the two-dimensional model in a

corresponding one-dimensional representation:

i Ai

< >A =

da

A i

(11)

da A

A

The reactor operation conditions and numerical parameters are presented in Table 1.

For both the SMR and SE-SMR processes, Figure 1 presents the one-dimensional and two-dimensional

model predictions of the dry mole fractions of CO, CO2, CH4 and H2 at the reactor outlet as a function of

time. Minor differences are observed in the prediction of the chemical reactor performance between the

one- and two-dimensional models. The differences in the simulation results obtained by the one- and two-

dimensional models the very first simulation seconds are related to the start-up of the multiphase reactive

flow algorithms. Nevertheless, the presence of the sorbent in the novel SE-SMR process significantly

favours the product side of the reformer and watergas-shift reactions (1)-(3), i.e., formation of H2,

relative to the commercial SMR process.

The dry mole fraction of CO2 and the temperature obtained by the one- and two-dimensional models;

as a function of the reactor length, are presented in figure 2 (SMR and SE-SMR). The prediction of the

dry mole fraction of CO2 of the SE-SMR process (Figure 2(a)) differs for the one- and two-dimensional

models close to the reactor inlet. However, except at the reactor entrance, only minor differences in the

CO2 concentration profiles are observed in the two model solutions. On the other hand, for the SMR

process (Figure 2(c)) the solutions obtained with the one- and two-dimensional models are almost

identical for the CO2 concentration. The deviation in the model predictions of the SMR and SE-SMR

processes must be related to the presence of the sorbent in the SE-SMR process; the mass transfer of CO2

between the gas and solid phases in the SE-SMR process influences on the source terms of the gas and

solid continuity equations. On the other hand; with extended conductivity fluxes according to Eq. (21),

good agreement between the two model solutions are obtained for the temperature profile within the SE-

SMR reactor (Figure 2(b)). The one-dimensional model temperature differences can be reduced by further

fitting the effective conductivity value to the two-dimensional model results. Moderately different bed

expansions are obtained with the one- and two-dimensional models giving temperature differences at the

transition zone between the dense bed and free board. Considering the SMR process (Figure 2(d)), the

one-dimensional model shows a larger temperature drop at the reactor entrance relative to the two-

dimensional model. Large convective mixing of solids is inherent in the two-dimensional model due to

the multidimensional macroscopic flow pattern.

J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294 289

Fig. 1. Dry mole fractions at the reactor outlet, i.e. z=H, as a function of time for CO, CO2, CH4 and H2. Simulation results of one-

dimensional model and cross-sectional average of two-dimensional model. SMR and Se-SMR processes.

290 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

Fig. 2. Simulation results of one-dimensional model and cross-sectional average of two-dimensional model. Temperature and dry

mole fraction of CO2. The SMR and SE-SMR processes. Simulation time: 40s.

Fig. 3. Area fraction of solid phase and gas phase velocity. The SMR process. Simulation results of one-dimensional model and

cross-sectional average of two-dimensional model. Simulation time: 40s.

J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294 291

dp (m) 20510-6

H (m) 0.7

out

p (Pa) 1.1105

s,mf (-) 0.6

t (s) 10-4

steam-to-carbon-ratio (-) 3

z (m) 0.01

dt (m) 0.1

3

p (kg/m ) 2000

vgs,in (m/s) 0.096

in

T (K) 873

p (-) 2.5

5. Conclusion

model describing gassolid flows within fluidized bed reactors. The reactive flow simulations of the SMR

and SE-SMR processes are compared with the results of a two-dimensional model. Validation of the one-

dimensional model is performed to elucidate whether the model can be reasonably adopted for simulation

of the two interconnected fluidized bed reactors with a dynamic solid flux transferred between the reactor

units. The dynamic solid circulation between fluidized beds units operated at different conditions is an

inherent requirement for the novel SE-SMR technology. Hence, a less computational demanding model to

study the performance of interconnected reactor units will be an important contribution to the progress of

the commercialization of circulating fluidized bed reactors intended for the SE-SMR technology.

The simulation results of the one-dimensional model are in good agreement with the two-dimensional

model considering the species concentration and temperature predictions of the SMR and SE-SMR

processes. On the other hand, fair deviations between the one- and two-dimensional models are observed

for the phase area fractions and the gas phase velocity. This deviation may be related to the gas bubble

effect that is not included in the one-dimensional model. For improved one-dimensional model solution,

the model should be further extended including the effect of gas by-pass in the dense solid bed.

292 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

References

[1] Koumpouras GC, Alpay E, Stepanek F. Mathematical modelling of low-temperature hydrogen production with in situ CO2

capture. Chem Eng Sci 2007;62:28332841.

[2] Wang Y, Chao Z, Jakobsen HA. Numerical study of hydrogen production by the sorption-enhanced steam methane

reforming process with online CO2 capture as operated in fluidized bed reactors. Clean Techn Environ Policy 2011;13:559565.

[3] Wang Y, Chao Z, Chen D, Jakobsen HA. SE-SMR process performance in CFB reactors: Simulation of the CO2

adsorption/desorption process with CaO based sorbents. Int J Greenhouse Gas Control 2011;5:489497.

[4] Wang Y, Chao Z, Jakobsen HA. 3D simulation of bubbling fluidized bed reactors for sorption enhanced steam methane

reforming processes. J Natural Gas Sci Eng 2010;2:105113.

[5] Lindborg H, Jakobsen HA. Sorption enhanced steam methane reforming process performance and bubbling fluidized bed

reactor design analysis by use of a two-fluid model. Ind Eng Chem Res 2009;480:13321342.

[6] Kunii D, Levenspiel O. Fluidization engineering. Boston: Butterworth-Heinemann; 1991.

[7] Jakobsen HA. Chemical reactor modeling: Multiphase reactive flows. Berlin Heidelberg: Springer-Verlag; 2008.

[8] Lun CKK, Savage SB, Jeffrey DJ. Kinetic theories for granular flow: inelastic particles in Couette flow and slightly inelastic

particles in general flow field. J Fluid Mechanics 1984;140:223256.

[9] Gidaspow D. Multiphase flow and fluidization. Continuum and kinetic theory descriptions. New York: Academic Press;

1994.

[10] Lindborg H, Lysberg M, Jakobsen HA. Practical validation of the two-fluid model applied to dense gas-solid flows in

fluidized beds. Chem Eng Sci 2007;62:58545869.

[11] Wang Y, Chao Z,Jakobsen HA. A sensitivity study of the two-fluid model closure parameters (,e) determining the main

gassolid flow pattern characteristics. Ind Eng Chem Res 2010;49:34333441.

[12] Satrio JA, Shanks BH, Wheelock TD. Development of a novel combined catalyst and sorbent for hydrocarbon reforming.

Ind Eng Chem Res 2005;44:39013911.

[14] Albrecht KO, Satrio JA, Shanks BH, Wheelock TD. Application of a combined catalyst and sorbent for steam reforming of

methane. Ind Eng Chem Res 2010;49:40914098.

[15] Chao Z, Wang Y, Jakobsen JP, Fernandino M, Jakobsen HA. Derivation and validation of a binary multi-fluid Eulerian

model for fluidized beds. Chem Eng Sci 2011;66:36053616.

[16] Carlo AD, Bocci E, Zuccari F, Dell'Era A. Numerical investigation of sorption enhanced steam methane reforming process

using computational fluid dynamics EulerianEulerian code. Ing Eng Chem Res 2010;49:15611576.

[17] Solsvik J, Jakobsen HA. A numerical study of a two property catalyst/sorbent pellet design for the sorption-enhanced

steam-methane reforming process: Modeling complexity and parameter sensitivity study. Chem Eng J 2011;178:407422.

[18] Rout KR, Solsvik J, Nayak AK, Jakobsen HA. A numerical study of multicomponent mass diffusion and convection in

porous pellets for the sorption-enhanced steam methane reforming and desorption processes. Chem Eng Sci 2011;66:41114126.

[19] Rout KR, Jakobsen HA. Reactor performance optimization by the use of a novel combined pellet reflecting both catalyst

and adsorbent properties. Fuel Process Technol 2012;99:1334.

[20] Xu J, Froment GF. Methane steam reforming, methanation and water-gas shift: I. Intrinsic kinetics. AIChE J 1989;35:

8896.

[21] Sun P, Grace JR, Lim CJ, Anthony EJ. Determination of intrinsic rate constants of the CaOCO2 reaction. Chem Eng Sci

2008;63:4756.

[22] Patankar SV. Numerical heat transfer and fluid flow. Hemisphere Publishing Corporation; 1980.

[23] Versteeg HK, Malalasekera W. An introduction to computational fluid dynamics: The finite volume method. 2nd ed.

London: Pearson Prentice Hall; 2007.

[24] Lindborg H. Modeling and simulations of reactive two phase flows in fluidized beds. Ph.D. thesis: The Norwegian

University of Technology and Science (NTNU); 2008.

[25] Wilke CR. Diffusional properties of multicomponent gases. Chem Engng Prog 1950;46:95104.

[26] Reid RC, Prausnitz JM, Poling BE. The properties of gases and liquids. New York: McGraw-Hill; 1987.

J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294 293

The constitutive equations adopted in the two-fluid model are presented in the sequent.

Stress:

vk

k = kt where t = 103 m , sm = 1 (12)

z

f k k vk vk

s ,wall = (13)

2

%g = %s = (vs vg ) (14)

s2 gm g | U g U s | s 3 C D | U g U s | g s g

2.65

g d p2 dp 4 dp

atan(150(g 1))

w= + 0.5 (16)

p )

CD = , Re p < 1000

Re p (17)

CD = 0.44, Re p >= 1000

gt

Dgeff,j = Dgm, j + (18)

g Sct

1 g , j 1

Dgm, j = (19)

Mg n g ,r

M

r =1 D jr

r

r j

294 J. Solsvik et al. / Procedia Engineering 42 (2012) 283 294

0.00266101325 Tg3/ 2

D jr = (20)

0.012 p jr 2jr M 1/jr 2

Effective conductivity:

t

kkeff = kkm + k t C with C = 105 (21)

k Pr

Molecular conductivity:

k gstat

k gm = (1 s ) (22)

g

k gstat

k sm = ( A + (1 )) (23)

s

=

2

[ A 1 2 B ln A B 1 1 ( B + 1)] (24)

1 B / A (1 B / A) A B 1 B / A 2

k sstat

A= (25)

k gstat

n

k gstat = y (

j

j j + jT + jT 2 + jT 3 ) (26)

10/9

B = 1.25 s (27)

g

= 7.26103 (28)

6s

Qgi = hgs (Ts Tg ) (29)

dp

Interfacial heat transfer coefficient:

kg

hgs = [(7 10

g + 5g2 )(1 + 0.7Re0.2

p Pr

1/3

) + (1.33 2.4g + 1.2g2 )Re0.7

p Pr

1/3

] (30)

dp

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